The multicolour three-photon resonant photoionization spectra and high-time-resolved laser spectrum of UI were measured with a setup composed of a Nd∶YAG-laser(532 nm, operated at 10 Hz)-pumped pulsed tunable dye laser system, a time-of-flight mass spectrometer, including micro-channel plate components, ns-oscilloscope, boxcar integrator, and so on. Creative inventions of this paper are for the first time by laser-induced quantum population of the graphic method, the causes for single-colour and two-colour three-photon resonant photoionization spectra peak were given in the three-colour three-photon resonant photoionization experiment； The question how to avoid producing single-colour and two-colour three-photon resonant photoionization spectra peak was solved, That is, how to solve the problem to avoid “false peaks”, so that multicolour three-photon resonant photoionization purity was raised remarkably; On this basis, not only in close proximity to energy level position with just a difference 0.642 cm-1, the isotopes A and B of uranium, which are difficult to distinguish, were well resolved, but the two excited state lifetime values were obtained respectively. This technology is not limited to uranium spectrum, but more importantly, it’s versatile. The new methods and technologies of basic research can be expanded to samples of biological and medical research fields with laser detecting and analysis.